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Degradation mechanism of surface coating effects at the cathode/electrolyte interface is investigated using thin-film model electrodes combined with operando X-ray absorption spectroscopy (XAS). MgO-coated LiCoO[2] thin-film electrodes prepared via pulsed laser deposition at room temperature and high temperature are used as model systems. The MgO coating improves the durability of the cathode during high-potential cycling. Operando total reflection fluorescence XAS reveals that initial deterioration due to reduction of Co ions at the surface of the uncoated-LiCoO[2] thin film upon electrolyte immersion is inhibited by the MgO coating. Operando depth-resolved XAS reveals that the MgO coating suppresses drastic distortions of local structure at the LiCoO[2] surface as observed in the uncoated-LiCoO[2] during charging process. The electronic and local structure changes at the electrode/electrolyte interface for two types of surface coating morphologies are discussed

Stabilization of the Electronic Structure at the Cathode/Electrolyte Interface via MgO Ultra-thin Layer during Lithium-ions Insertion/Extraction